Second-order spectral lineshapes from charged interfaces

Second-order nonlinear spectroscopy has proven to be a powerful tool in elucidating key chemical and structural characteristics at a variety of interfaces. However, the presence of interfacial potentials may lead to complications regarding the interpretation of second harmonic and vibrational sum frequency generation responses from charged interfaces due to mixing of absorptive and dispersive contributions. Here, we examine by means of mathematical modeling how this interaction influences second-order spectral lineshapes. We discuss our findings in the context of reported nonlinear optical spectra obtained from charged water/air and solid/liquid interfaces and demonstrate the importance of accounting for the interfacial potential-dependent χ(3) term in interpreting lineshapes when seeking molecular information from charged interfaces using second-order spectroscopy. Charged interfaces are important in chemical systems, but the influence of charge on vibrational sum frequency spectra has only recently been considered. Here the authors show the importance of accounting for the interfacial potential-dependent χ(3) term in interpreting spectral lineshapes from charged interfaces.

• Publication year

  2017

• Venue

  Nature Communications

• Publication date

  2017-03-10

• Fields of study

  Materials Science, Physics, Chemistry, Medicine

• Identifiers
  DOI 10.1038/s41467-017-01088-0arXiv 1703.03686PMID 29044095PMCID 5647331
• External record

  Open on Semantic Scholar

• Source metadata

  Semantic Scholar, PubMed

• No claims are published for this paper.

• No concepts are published for this paper.

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